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The mutual promotion of photolysis and laccase-catalysis on removal of dichlorophen from water under simulated sunlight irradiation
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2018-01-05 , DOI: 10.1016/j.cej.2018.01.026
Huanhuan Shi , Guowei Wang , Qingguo Huang , Jianhua Li , Yun Yang , Shixiang Gao , Zunyao Wang

The combined removal of dichlorophen (DDM) by photolysis and laccase-catalysis in aqueous solution under simulated sunlight irradiation was investigated. It was found that DDM could be effectively degraded under simulated sunlight irradiation, which was triggered primarily by singlet/triplet state (1DDM/3DDM). The photolysis process of DDM is highly pH-dependent, mainly because of the change in electronic density distribution on the aromatic ring of DDM in its varied ionic speciation under different pH. The significant role of singlet oxygen (1O2) and 3DDM in DDM photolysis was verified by experimental measurements and density functional theory (DFT) calculation. The combination of photolysis and laccase-catalysis processes can promote the removal of DDM synergistically. Product identification revealed that photolysis and laccase-catalysis attacked DDM molecule at different moieties. Single aromatic ring products were formed via photo-oxidation of DDM by 1O2. Meanwhile, photolysis can efficiently remove the oxidative coupling products of DDM formed in laccase-catalysis process, which are considered to be potentially high toxic products. In addition, this study also provided first evidence of the laccase inactivation mechanisms induced by simulated sunlight, namely, the destruction of copper catalytic centers and secondary structure.



中文翻译:

模拟阳光照射下光解和漆酶催化的相互促进作用,从水中去除二氯酚

研究了在模拟阳光照射下水溶液中光解和漆酶催化联合去除二氯苯酚(DDM)的能力。发现在模拟的阳光照射下DDM可以有效降解,这主要是由单重态/三重态(1 DDM / 3 DDM )触发的。DDM的光解过程高度依赖于pH值,这主要是由于在不同pH下DDM的各种离子形态中DDM芳环上电子密度分布的变化。单线态氧(1 O 2)和3 DDM *的重要作用通过实验测量和密度泛函理论(DFT)的计算验证了DDM中的光解作用。光解和漆酶催化过程的结合可以协同促进DDM的去除。产品鉴定表明,光解和漆酶催化攻击了不同部分的DDM分子。通过DDM被1 O 2光氧化形成单个芳香环产物。同时,光解可以有效地去除漆酶催化过程中形成的DDM的氧化偶合产物,该产物被认为是潜在的高毒性产物。此外,这项研究还提供了模拟阳光诱导的漆酶失活机制的第一个证据,即铜催化中心和二级结构的破坏。

更新日期:2018-01-05
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